Methods for forming metal-containing particles in barton reactors and for retrofitting barton reactors

ABSTRACT

According to one or more embodiments presently described, metal-containing particles may be formed by a method including forming a molten material from a solid supply material, introducing the molten material into a reaction zone of a Barton reactor, and contacting the molten material with a processing gas in the reaction zone to form solid metal-containing particles comprising solid metallic particles and solid metal oxide particles. The Barton reactor may include a reaction vessel which may include a top cover and sidewalls defining the reaction zone, an agitator, a processing gas inlet, and a product outlet. The molten material may be introduced to the reaction zone in a laminar flow or as atomized molten particles. Less than 99% of the particles may include metal oxide.

CROSS-REFERENCE TO RELATED CASES

The present application claims priority to U.S. Provisional ApplicationNo. 62/616,593, filed Jan. 12, 2018, entitled “METHODS AND SYSTEMS FORPRODUCING METAL-CONTAINING PARTICLES”, and claims priority to U.S.Provisional Patent Application Ser. No. 62/743,698, filed Oct. 10, 2018,entitled “METHODS AND SYSTEMS FOR PRODUCING METAL-CONTAINING PARTICLES”,each of which are incorporated by reference in their entirety herein.

BACKGROUND Field

The present disclosure relates to methods and systems for producingmetal-containing particles and, more particularly, to methods andsystems for converting source metal-containing materials intometal-containing solid particles.

Technical Background

Powdered pure metals and/or metal oxides are utilized in a wide varietyof manufacturing and material formation. For example, mixtures of leadoxide and pure lead may be utilized in the manufacture of lead acidbatteries. Other metal powders may be utilized in the formation of bulkmetals and tools, such as through sintering or other alloy formationtechniques. Additionally, pure or alloy metal particles may be utilizedas additives in paints, coatings, lubricants, or X-Ray shielding.

BRIEF SUMMARY

Accordingly, there is a need for improved methods and systems for makingsuch particles. One or more of the presently disclosed embodimentsrelate to systems and/or methods for processing metal-containingmaterials into particle-sized, metal-containing materials (e.g.,powders) having either the same or a different chemical composition asthe source metal-containing material. For example, molten feed metalsmay be processed into solid particulates of pure metals, alloys, ormetal oxides. In one or more embodiments, metals such as lead may bechemically processed by changing the composition (such as into leadoxide) or may be physically changed by changing the shape, size, orcrystal structure. For example, lead metal may be processed to formpowdered lead oxides having one or more crystal morphologies throughmechanical and chemical means. The formation of non-lead metals andmetal oxides is also contemplated by the presently disclosed methods andsystems.

According to one or more embodiments, metal-containing particles may beformed by a method comprising forming a molten material from a solidsupply material, introducing the molten material into a reaction zone ofa Barton reactor, and contacting the molten material with a processinggas in the reaction zone to form solid metal-containing particlescomprising solid metallic particles and solid metal oxide particles. TheBarton reactor may comprise a reaction vessel which may comprising a topcover and sidewalls defining the reaction zone, an agitator, aprocessing gas inlet, and a product outlet. The molten material may beintroduced to the reaction zone in a laminar flow or as atomized moltenparticles. Less than 99% of the particles may comprise metal oxide.

According to one or more additional embodiments, a Barton reactor may beretrofitted by a method comprising replacing a conventional moltenmaterial inlet of a Barton reactor with an injector operable to receivemolten material and inject the molten material into a reaction zone ofthe Barton reactor. The injector may be operable to pass moltenmetal-containing material into the reaction zone with a laminar flow orin an atomized form.

Additional features and advantages of the technology described in thisdisclosure will be set forth in the detailed description which follows,and in part will be readily apparent to those skilled in the art fromthe description or recognized by practicing the technology as describedin this disclosure, including the detailed description which follows,the claims, as well as the appended drawings.

BRIEF DESCRIPTION OF THE DRAWINGS

The following detailed description of specific embodiments of thepresent disclosure can be best understood when read in conjunction withthe following drawings, where like structure is indicated with likereference numerals and in which:

FIG. 1 schematically depicts a side view of a Barton-style system usedfor forming metal-containing particles, according to one or moreembodiments described herein;

FIG. 2 schematically depicts a top view of the system of FIG. 1,according to one or more embodiments described herein;

FIG. 3 schematically depicts a perspective side view of another systemused for forming metal-containing particles, according to one or moreembodiments described herein;

FIG. 4 schematically depicts a perspective top down view of the systemfor forming metal-containing particles of FIG. 3, according to one ormore embodiments described herein;

FIG. 5 schematically depicts a side view of a molten material reservoirand injector, according to one or more embodiments described herein;

FIG. 6 schematically depicts a side view of a molten material injector,according to one or more embodiments described herein;

FIG. 7A schematically depicts a cross-sectional side view of asingle-conduit injector, according to one or more embodiments describedherein;

FIG. 7B schematically depicts a cross-sectional side view of asingle-conduit injector, according to one or more embodiments describedherein;

FIG. 8 schematically depicts a top-down view of the atomization nozzleof FIG. 6 or 7A, according to one or more embodiments described herein;

FIG. 9 schematically depicts a bottom-up view of the gas manifold shownin FIG. 6, according to one or more embodiments described herein;

FIG. 10 schematically depicts a side view of a system used for formingmetal-containing particles that includes a molten material reservoir,according to one or more embodiments described herein;

FIG. 11 schematically depicts a side view of a multi-conduit reactor,according to one or more embodiments described in this disclosure;

FIG. 12 schematically depicts a top view of the multi-conduit reactor ofFIG. 11, according to one or more embodiments described in thisdisclosure;

FIG. 13 schematically depicts a reactor system that includes amulti-conduit reactor, according to one or more embodiments described inthis disclosure;

FIG. 14 depicts a mathematical model relevant to producingmetal-containing particles in a multi-conduit injector, according to oneor more embodiments described in this disclosure;

FIG. 15 depicts another mathematical model relevant to producingmetal-containing particles in a multi-conduit injector, according to oneor more embodiments described in this disclosure; and

FIG. 16 depicts another mathematical model relevant to producingmetal-containing particles in a multi-conduit injector, according to oneor more embodiments described in this disclosure.

It should further be noted that in some figures, such as FIG. 13, arrowsin the drawings may refer to process streams. However, the arrows mayequivalently refer to transfer lines which may serve to transfer processsteams between two or more system components. Additionally, arrows thatconnect to system components define inlets or outlets in each givensystem component. The arrow direction corresponds generally with themajor direction of movement of the materials of the stream containedwithin the physical transfer line signified by the arrow. Furthermore,arrows which do not connect two or more system components signify asystem product stream which exits the depicted system or a system inletstream which enters the depicted system. System product streams may befurther processed in accompanying chemical processing systems or may becommercialized as end products. System inlet streams may be streamstransferred from accompanying chemical processing systems or may benon-processed feedstock materials.

Additionally, arrows in the drawings may schematically depict processsteps of transporting a stream from one system component to anothersystem component. For example, an arrow from one system componentpointing to another system component may represent “passing” a systemcomponent effluent to another system component, which may include thecontents of a process stream “exiting” or being “removed” from onesystem component and “introducing” the contents of that product streamto another system component.

For the purpose of describing the simplified schematic illustrations anddescriptions of FIGS. 1-13, the numerous valves, temperature sensors,electronic controllers and the like that may be employed and well knownto those of ordinary skill in the art of certain chemical processingoperations are not included. Further, accompanying components that areoften included in conventional chemical processing operations are notdepicted. It should be understood that these components are within thespirit and scope of the present embodiments disclosed. However,operational components, such as those described in the presentdisclosure, may be added to the embodiments described in thisdisclosure.

Reference will now be made in greater detail to various embodiments,some embodiments of which are illustrated in the accompanying drawings.Whenever possible, the same reference numerals will be used throughoutthe drawings to refer to the same or similar parts.

DETAILED DESCRIPTION

The present application, according to one or more embodiments, isdirected to methods and/or systems utilized in the formation ofmetal-containing particles. It has been discovered that the introductionof a molten metal-containing material in an atomized form (i.e.,comprising liquid particles), or with a laminar flow, may have severaladvantages for producing metal-containing particles as compared withconventional methods which generally utilize the introduction of a bulkliquid stream of molten metal-containing material into a reactor such asa Barton. For example, conventional processes may utilize theintroduction of molten material into a reactor from the end of a pipe ina non-laminar, turbulent flow. For example, according to one or moreembodiments disclosed herein, the introduction of the moltenmetal-containing material in an atomized or laminar form may providemore reactive surface area, and therefore enhance the oxidation rate ofreaction, and correspondingly enhance the production rate of metaloxides, such as lead oxide. The incorporation of a controlled, atomizedor laminar molten feed stream into the reactor may enhance control ofthe physical characteristics (e.g., particle size), chemicalcharacteristics (e.g., average oxidation state, crystal morphology)and/or the product manufacturing rates of the metal-containingparticles. For example, it is contemplated that atomization of a moltenmetal-containing material may be performed by injection of the moltenmetal-containing material from an atomizing injector which may directlyatomize the molten metal-containing material when it is passed out of anozzle (for example, a misting nozzle), or may pass a laminar flow ofmolten metal-containing material out of a nozzle which is subsequentlyatomized by impingement with a flow of relatively high velocity gas. Inother embodiments, a laminar flow of molten metal-containing materialmay improve process output as compared with a similar process thatintroduces the molten metal-containing material through a conventionalpipe source. Additionally, the molten metal-containing material may bepassed from a nozzle in a laminar flow pattern which increases thesurface area to volume ratio of the molten metal-containing material,allowing for increased contact with surrounding gasses. For example, ahollow cone laminar flow pattern may be utilized which increases thesurface to volume ratio of the molten metal-containing material as it isexpelled from the injector and enters the reactor. In additionalembodiments the laminar flow pattern may sufficiently increase thesurface area to volume ratio of the molten metal-containing material (ascompared with introduction by a pipe or simple trough overflow scheme)such that when the laminar molten metal-containing material is contactedby an agitator it atomizes. These and other aspects of the presentlydisclosed technology are described herein in the context of systems andmethods which may be utilized to form metal-containing particles.

According to one or more embodiments, by any of the methods or systemspresently disclosed, a mixture of lead metal particles (sometimes called“free lead”) and lead oxide particles may be formed. In some embodimentspresently disclosed, the weight ratio of formed solid lead oxideparticles to solid lead metal particles may be less than 99:1. Forexample, the particles formed by the presently disclosed methods mayhave a weight ratio of formed solid lead oxide particles to solid leadmetal particles of from 50:50 to 99:1 (such as from 50:50 to 60:40, from60:40 to 70:30, from 70:30 to 80:20, from 80:20 to 90:10, or from 90:10to 99:1, or combinations thereof) or any combination thereof). Inadditional embodiments, the weight ratio of formed solid lead oxideparticles to solid lead metal particles may be from 50:50 to 90:10, suchas form 50:50 to 85:15. Such ratios may be well suited for lead acidbatteries. However, it is contemplated that other ratios may be utilizedfor lead acid batteries as well. In additional embodiments, a majorityby weight of the product is metallic lead (e.g., the product comprisesat least 75 wt. %, at least 90 wt. %, at least 95 wt. %, or even atleast 99 wt. % of metallic lead particles (non-oxidized).

In one or more embodiments, the lead oxide formed may be majority byweight alpha lead oxide having a tetragonal crystal structure. Forexample, at least 50 wt. %, at least 60 wt. %, at least 70 wt. %, atleast 80 wt. %, at least 90 wt. %, at least 99 wt. %, or even at least99.9 wt. % of the formed lead oxide may be alpha lead oxide. In suchembodiments, a minority of the formed lead oxide may be beta lead oxidehaving an orthorhombic crystal structure. For example, less than 50 wt.%, 40 wt. %, 30 wt. %, 20 wt. %, 10 wt. %, or even 1 wt. % of the formedlead oxide may be beta lead oxide. However, in additional embodiments, amajority by weight of beta lead oxide is contemplated. It should beunderstood that mixtures of free lead and lead oxide, where the majorityby weight of the lead oxide is alpha lead oxide, may be suitable forlead acid batteries. For example, in one or more embodiments, the weightratio of formed solid lead oxide particles to solid lead metal particlesof from 50:50 to 99:1 and the majority by weight of the lead oxide maybe alpha lead oxide. In additional embodiments, the weight ratio offormed solid lead oxide particles to solid lead metal particles of from50:50 to 90:10 and at least 90 wt. %, or even 99 wt. % of the lead oxidemay be alpha lead oxide.

In one or more embodiments, the reaction to form lead oxide may takeplace at from 621° F. (about the melting point of lead) to 850° F. oreven to 880° F. (e.g., from 621° F. to 700° F., from 700° F. to 800° F.,from 800° F. to 850° F., from 850° F. to 880° F., or combinationsthereof). Such temperatures may be suitable for forming majority byweight alpha lead oxide and/or allowing for at least 1 wt. % of theproduct to remain as metallic lead (i.e., not converted to lead oxide).Without being bound by theory, it is believed the higher processingtemperatures may lead to almost total conversion of lead to lead oxide(e.g., greater than 99 wt. % lead oxide as product) and/or the formationof majority by weight beta lead oxide. Such temperatures (from 621° F.to 880° F.) may be suitable for forming lead oxide which can be utilizedin lead oxide batteries.

According to additional embodiments, a majority of the produced leadoxide is beta lead oxide. For example, at least 50 wt. %, at least 60wt. %, at least 70 wt. %, at least 80 wt. %, at least 90 wt. %, at least99 wt. %, or even at least 99.9 wt. % of the formed lead oxide may bebeta lead oxide. In such embodiments, free lead may be present in theproduct in amounts of at least 1 wt. %, at least 2 wt. %, at least 5 wt.%, at least 10 wt. %, at least 20 wt. %, or even at least 50 wt. %. Itis contemplated that reactor temperatures of greater than 880° F. may beutilized in some embodiments, such as when beta lead is a desiredproduct.

It should be understood that one or more embodiments of the presentdisclosure are directed to molten material injectors (sometimes referredto herein as injector devices) that may be compatible for use with aBarton reactor. For example, according to some embodiments, aconventional Barton reactor that utilizes a non-atomized or non-laminarflow of molten metal-containing material into the conventional Bartonpot (e.g., by passing the molten metal-containing material into theBarton pot through a stand pipe or the like) may be enhanced byretrofitting the conventional Barton reactor with the molten materialinjectors presently described herein. The use of the presently describedmolten material injectors may improve product output, among otherdesirable results. However, it is contemplated that the disclosedinjectors may be incorporated into a wide variety of reactor types, ofwhich several non-limiting examples are provided herein.

As described herein, “metal-containing” materials include any materialswhich comprise a metal or metalloid element. For example,metal-containing materials include metal oxides, metal alloys, orsubstantially pure metallic materials. Pure or near pure metals (e.g.,those comprising at least 99 wt. %, 99.5 wt. %, 99.9 wt. %, or even99.99 wt. % of a single element) may be referred to as “metallic,” suchas “metallic lead” or “metallic aluminum”, etc., or simply as “metal,”such as “lead metal” or “aluminum metal.” Furthermore, as describedherein, “pure metals” and “alloys” are non-oxidized (i.e., contain lessthan 1% of molecules oxidized). While the formation of particlescomprising any metal-containing materials are presently contemplated inthis disclosure, the conversion of lead to lead oxide is described withreference to several of the herein disclosed embodiments. As such, someembodiments disclosed herein may be described with respect to theproduction of lead oxide from metallic lead. However, it should beappreciated that similar methods and systems for the production ofnon-lead materials may be utilized within the scope of the presentdisclosure. By way of example, metals processed by the methods andsystems disclosed herein may include lead, bismuth, aluminum, zinc,nickel, antimony, alloys thereof, and oxides thereof.

Additionally, as described herein, “particles” or “particulate form” mayrefer to solid or liquid matter in discrete bodies with diameters of1000 microns or less (such as 500 microns or less, 400 microns or less,300 microns or less, 200 microns or less, 100 microns or less, 50microns, 25 microns or less, or even smaller). For example, the vastnumber of formed solid particles by the presently disclosed processesmay fit through a No. 50 mesh US standard sieve and have a diameter of300 microns or less. However, some particles may be much smaller thanthose having a diameter of 300 microns or less. For example, the d₅₀ ofthe particles formed by the presently disclosed processes may be from 1to 5 microns, from 5 microns to 10 microns, from 10 microns to 25microns, from 25 microns to 50 microns, from 50 microns to 100 microns,from 100 microns to 150 microns, from 150 microns to 200 microns, from200 microns to 250 microns, from 250 microns to 300 microns, or anycombination thereof. In one or more embodiments, a lead oxide particlesmay be formed where 95 wt. % of the lead oxide particles has a diameterof 100 microns or less. In one or more embodiments, a metallic leadparticles may be formed where 95 wt. % of the lead particles have adiameter of 1000 microns or less. Molten materials in particle form maybe referred to as “atomized,” or being in an “atomized form.” Alsocontemplated herein are embodiments where only a portion of the moltenfeed is atomized. It should be understood that “atomized” moltenmaterials may refer to molten materials that are in particulate liquidor droplet form. For example, according to some embodiments, at least 50vol.%, at least 60 vol.%, at least 70 vol.%, at least 90 vol.%, or evenat least 95 vol.% of the molten material injected into the reactor mayhave be in discrete bodies having a diameter of 1000 micron or less.

As used herein, a “chemical change” refers to a change which affects thechemical composition of a material. For example oxidation of a metal oralloy in the feed stream to form a metal oxide is considered a chemicalchange. Additionally, as used herein, a “physical change” refers to achange affecting the form of a chemical substance, but not its chemicalcomposition. Examples of physical changes include changes in size,shape, phase, etc. It should be understood that, in some embodiments, achemical and physical change may take place. However, in otherembodiments, a chemical change may not take place. For example, thecontents of the feed stream may be powderized, but maintain theirchemical composition. Without being bound by theory, it is believed thatthe contents of the fluid stream may at least partially determinewhether a chemical change takes place. For example, a fluid streamcomprising oxygen may allow for combustion, forming metal oxides, but aninert fluid stream such as nitrogen may not alter the composition of themetal or alloy in the feed stream, as will be discussed in detailherein. Additionally, without being bound by theory, it is believed thatparticular characteristics of the fluid stream, such as its momentumflux relative to that of the feed stream may atomize the metal or alloypresent in the feed stream, resulting in the formation of powderizedmetals, alloys, and/or oxides thereof in the product stream.

As used herein, “atomizing” a material refers to converting a bulkmaterial into fine particles or droplets. For example, a metal or alloyincluded in the feed stream may be atomized into fine particles whencontacted by the fluid stream.

As compared with one or more embodiments of the presently disclosedsystems, a conventional Barton reactor may be an inefficient atomizer(e.g., by means of its agitator blade as described subsequently herein),producing particles with a larger than desired particle sizedistribution. As described herein, a “conventional Barton” reactorrefers to one which introduces molten metal by pipe, overflow or atrough, or similar means (i.e., not by the injectors presentlydisclosed). A “modified Barton” may be referred to herein and includessome means for introducing the molten metal in an atomized or laminarflow form. However, it should be understood that a “modified Barton” mayrefer to a Barton-style reactor which was not previously fitted with apipe style injector and then retrofitted. For example, the presentdescription is intended to include Barton reactors which were originallyfitted with the injectors presently disclosed.

In one or more embodiments of conventional Barton operation, theagitator atomizes a portion of the lead feed in an atmosphere whichallows the oxidation of lead particles. Some of the lead oxide remainsin the bath until its particle size is small enough to allow it to beconveyed out of the reactor. When the conventional Barton reactor isoperating in a steady state there is a mixing of lead and lead oxidewhich is also conducive to oxidation. Atomization may be needed to getrapid oxidation. Molten lead on the surface of the melt kettle oxidizesslowly over hours of operation. Molten lead from the injector does notappear to oxidize until the lead film breaks into small particles. Assuch, in one or more embodiments, the Barton agitator does atomize asignificant portion of the lead feed but it is not an efficient atomizerand it produces a wider variation in particle size distribution by thenature of the lead feed and the lead feed's point of impact on theagitator. The presently disclosed embodiments may directly introduce themolten metal as a particulate or in laminar flow, which may generategreater contact and reaction between the molten materials and processfluids such as air.

Referring now to FIG. 1, a modified Barton reactor system utilized toform metal-containing particles is depicted. According to one or moreembodiments, the reactor system 100 may include a reactor 101, a moltenmaterial injector device 300, and a molten metal-containing materialsource 162. According to one or more embodiments, moltenmetal-containing material may be fed from the molten metal-containingmaterial source 162 to the molten material injector device 300. Themolten material injector device 300 may inject the moltenmetal-containing material into the reactor 101, where it is processedinto solid metal-containing particles, such as lead particles, leadoxide particles, or both.

The molten metal-containing material source 162 may comprise pipingwhich is fluidly connected to a melt kettle (not depicted in FIG. 1) orother apparatus which may melt solid metal-containing supply materials.For example, the melt kettle may melt solid metallic lead into moltenlead. A valve may control the flow of the molten metal-containingmaterial. In some embodiments, the molten material may be conveyed witha pump (such as a pump submerged in a melt kettle). In additionalembodiments, the molten material may be conveyed by gravity alone, or atleast in part. According to one or more embodiments, metal, such aslead, may be melted in the melt kettle to a temperature at or exceedingthe metal's melting point, such as about 621° F. for lead, and less thanthat of the metals boiling point, such as about 3,180° F. for lead.Without limitation, in one embodiment, the molten material may be pumpedfrom the melt kettle through a pipe directly to the molten materialinjector device 300.

Moreover, and as described herein, conventional Barton processes providea stream of molten lead through a pipe, trough, or other likeintroduction device from a melting kettle leading to a Barton Reactor. Atrough design may be similarly referred to as a “dam” or “lip” wheremolten metal spills over a raised wall and into the Barton or otherreactor. In one or more embodiments presently described, such trough,dam, lip, or like device is not utilized. The molten lead flow inconventional Barton processes is typically controlled with a manualvalve that is submerged in the melting kettle or a lead pump. Such apump may be submerged below the surface of the molten metal adjacent tothe area where bars of lead are fed into the melting kettle. The massflow rate of molten lead feeding into the Barton reactor can be modifiedby controlling the pump's rpms. As the melt kettle is depleted of moltenlead, it is replenished with solid bars of lead that subsequently meltand increase the level of molten lead. As the stream of molten lead isintroduced into the Barton reactor, the distance between the end of thepipe and the Barton agitator may be relatively small and insufficient toallow the major portion of the fluid stream to break up and form moltenlead droplets or atomize. Additionally, the relative velocity of the airsurrounding the molten stream of lead is generally inadequate to promoteatomization. Likewise, the mass flowrate of the molten lead stream isirregular and does not promote the formation of liquid droplets.Additionally, the process of repeatedly adding solid bars of lead intothe melting kettle introduces both temperature and mass flow ratevariation to the molten stream of lead. When a solid bar of lead isintroduced into the melting kettle, the temperature of the molten leaddrops as the solid lead component absorbs thermal energy. Once the solidlead has completely been melted, the temperature rises to a prescribedtemperature. As the level of molten lead rises and falls, the headpressure at the lead pipe inlet changes and therefore continuouslychanges the mass flow rate of molten lead delivered to the Bartonreactor. Such deficiencies may be overcome by the embodiments describedherein.

Some embodiments, as depicted in FIG. 1, may utilize a molten materialpump 165 to provide sufficiently pressurized molten metal-containingmaterial to the molten material injector device. It should beappreciated that the system of FIG. 1 may operate with any of the moltenmaterial injector devices 300 described herein, and that the moltenmaterial pump 165 may be sufficient in one or more embodiments tomaintain a relatively constant pressure of molten metal-containingmaterial to the molten material injector device 300 such that the flowof molten metal-containing material into the reactor 101 is relativelyconstant and at a pressure sufficient to atomize and/or form a laminarflow pattern on the molten metal-containing material.

In some embodiments, the molten material injector device 300 maycomprise a gas manifold, as described in additional detail hereinbelow.The air manifold may be directly connected to a gas supply 132. Itshould be understood that the molten material injector device 300 of thesystem of FIG. 1 may be utilized with a reservoir 161 (as is depicted inFIG. 10 and subsequently described herein) or with a pump such as in theembodiment of FIG. 1.

According to one or more embodiments, the reactor 101 may include abottom bowl 103, a top cover 106, and sidewalls 104 defining a reactionzone 108. As depicted in the embodiments of FIGS. 1 and 2, the reactor101 may be cylindrically shaped, although other shapes are contemplatedsuch as, for example, a dome shape. The reactor 101 may additionallyinclude a gas inlet 122 and a water inlet 124. An oxidizing gas such asair, may enter the reactor 101 via the gas inlet 122, an inert gas suchas nitrogen, may enter the reactor 101 via the gas inlet 122. Theproduct material (i.e., solid metal-containing particles) may exit thereactor 101 through a solid metal-containing material outlet 126. Themetal-containing material outlet may comprise, for example a duct,chute, or other passage. The gas may pass into the reaction zone 108 viagas inlet 122 and may pass out of the reaction zone 108 (along with thesolid particle products) via solid metal-containing material outlet 126.The gas exiting through the solid metal-containing material outlet 126gas may at least partially aid in transporting the solid particles outof the reactor 101. The reactor 101 may additionally include a waterinlet 124. Water may be injected into the reaction zone 108 to controlthe temperature in the reaction zone 108. It should be understood thatwhile FIGS. 1 and 2 depict one embodiment of a reactor suitable for thepresently described processes, other reactor configurations arecontemplated, such as reactor configurations with varying geometricshapes and positions for the one or more inlets and outlets of thereactor. For example, the molten material injector device 300 may bepositioned on a sidewall 104 of the reactor 101.

The reactor 101 includes a reaction zone 108 where a reaction orphysical change to the molten material takes place. As described herein,the “reaction” may include any chemical or physical change of theinjected molten metal-containing material. For example, the moltenmetal-containing material may be oxidized in the reaction zone 108.However, in other embodiments, the molten metal-containing material maynot undergo a chemical reaction, and may instead be converted to solidparticles of a similar or smaller size than the molten metal-containingmaterial entering the reactor 101. For example, an oxidation reactionmay take place when an oxidizing gas, such air, is injected into thereactor 101. However, nitrogen or other non-reactive gasses may beutilized when oxidation is not desired. It should further be appreciatedthat the use of an oxidizing gas may yield both oxidized and metallicproduct in a mixture. It is contemplated that in any embodimentdescribed herein which generates a metal oxide by exposure to oxygen,air, pure oxygen, or any combination or mixture thereof may be utilized.For example, molar ratios of air to oxygen of about 10:0, 7.5:2.5, 5:5,2.5:7.5 and 0:10 are contemplated.

The reactor 101 may include, in some embodiments, an agitator 114, suchas a blade The blade may rotate to mix and agitate moltenmetal-containing materials passed into the reactor 101. The agitator 114may be driven by the rotation of a rotor 112, where one or moreappendages spin to agitate the molten material in the reactor 101.

FIG. 1 depicts a Barton reactor (sometimes referred to as a Barton pot),such as disclosed in in U.S. Pat. No. 633,533. In one or moreembodiments presently disclosed, a Barton reactor may be modified by theaddition of a molten material injector device 300. In a conventionalprocess utilizing a Barton reactor, a large heated pot may be fed with astream of molten lead (non-atomized) which is maintained at a shallowdepth in the bottom of the pot. A rapidly rotating blade in the bottomof the pot may continuously agitate the molten lead, which is oxidizedin the presence of a stream of air and water or steam. A portion of theoxidized lead particles and/or atomized lead droplets may be drawn fromthe pot by the air stream while the heavier lead droplets fall bygravity to the bottom of the pot for further agitation and oxidation.The process may be controlled by adjusting the rate of feed of themolten lead, the air flow through the pot, and/or the speed of theblade. In one or more embodiments, a Barton process may operate atrelatively high temperatures, substantially above the melting point oflead which is 327° C. (621° F.) when oxidized lead is desired.

Conventional Barton reactors and processes (without the modificationsdescribed herein) may have several inherent disadvantages to theprocesses described herein utilizing an atomized or laminar flowintroduction of molten metal. For example, when used for producing highfree lead litharge for battery manufacturing, the lead oxides producedare often too coarse for use in the formulation of battery activematerial paste and must, therefore, be subjected to hammer millprocessing subsequent to their initial production in a Barton pot. Inaddition, the conventional Barton process may be difficult to controlwhen used to produce low free lead litharge and may not be capable ofconsistently producing lead oxide with a free lead content of less than1 wt. % (or even with a free lead content of less than 2 wt. %, 3 wt. %,4 wt. %, 5 wt. %, 10 wt. %, 15 wt. %, 20 wt. %, 25 wt. %, 30 wt. %, 35wt. % or even 40 wt. %). Additionally, the operation of a conventionalBarton pot may result in a build-up of lead on the blade and walls,requiring periodic shut down and manual cleaning of the componentsurfaces.

According to some of the embodiments presently disclosed, a Barton orBarton-type reactor is not utilized for the formation of the particles.As would be appreciated by one skilled in the art, Barton reactors maybe utilized to form lead oxides. However, it has been discovered, as isdescribed herein, that other reactor configurations may be utilized toform metal-containing particles. In one or more embodiments, thesepresently described reactors may form particles through contact with aninjected stream of molten metal with a process gas in a reactor prior tothe molten metal contacting the bottom of the reactor.

Referring now to FIG. 3, a side perspective view of a reactor system 200utilized to form metal-containing particles is depicted. According toone or more embodiments, the reactor system 200 may include a reactor201 defining a reaction zone 220. The reactor system 200 may include aseparation zone 202 generally downstream of the reactor 201. A moltenmaterial may be supplied to the reactor 201 via a molten metal materialsupply system 260, and subsequently through a molten material injectordevice 300. A gas may be supplied to the reactor 201 by a gas supplysystem 270. The molten material injector device 300 may generallypositioned on an upper portion of the reaction zone 202 and pass themolten material downwardly. The process gas may enter the reaction zonethrough one or more inlets that are tangential to the perimeter of thereaction zone, allowing for the process gas to swirl around theperimeter of the reaction zone tangential to the sidewalls. For example,a cyclonic processing gas pattern may be formed around the perimeter ofthe reaction zone. The injector 300 may be positioned near the center ofthe upper portion of the reaction zone 202 such that the process gasswirls around the perimeter of the reaction zone 202 and contacts themolten material as it passes through the reaction zone 202.

According to one or more embodiments, as is described herein, the moltenmetal is injected into the reactor 201 and is contacted by a processgas, which forms a solid, metal-containing particle. The solid particlesare collected in the separation zone 202 where the various reactiongases are separated from the particles. The reactor zone may operate attemperatures of at least 621° F., such as temperatures contemplated inother reactor embodiments and described herein. The separation zone mayhave a lower temperature, such as below the melting point of material ofthe formed particles, such as 621° F. for lead.

According to one or more embodiments, the molten metal material supplysystem 260 may include a molten metal material source 262, a moltenmetal material pump 265, and a molten metal material supply line 263.The molten metal material supply line 263 may be in fluid communicationwith the molten material injector device 300. The molten metal materialsource 262 may be in fluid communication with a source of molten metal,such as a kettle. In other embodiments, the molten metal material may besupplied to the molten material injector device 300 at an appropriateand consistent pressure using other means such as a gravity pressurizedreservoir. The molten material injector device 300, which is explainedin detail below, injects the molten metal into the reactor 201.

The molten metal material source 262 may comprise piping which isfluidly connected to a melt kettle (not depicted in FIG. 3) or otherapparatus which may melt solid metal-containing supply materials. Forexample, the melt kettle may melt solid metallic lead into molten lead.In additional embodiments, the molten material may be conveyed bygravity alone, or at least in part. According to one or moreembodiments, metal, such as lead, may be melted in the melt kettle to atemperature at or exceeding the metal's melting point, such as 621° F.for lead, and less than that of the metals boiling point, such as 3,180°F. for lead. Without limitation, in one embodiment, the molten materialmay be pumped from the melt kettle through a pipe into the reservoir(not shown) or directly to the molten material injector device 300.

The reactor 201 may define a reaction zone 220, and may include an uppersection 223 having a circular cross section, such as a cylindricalshape, with a defined height and diameter, and a lower frustum section205 with a defined height and lower opening diameter. Gas may besupplied to the upper cylindrical section 223 using a gas supply system270. According to some embodiments, the gas supply system 270 mayinclude a blower 271, a gas inlet 272, and a gas injection line 273.According to some embodiments, the gas supply system 270 may beconfigured to supply an oxidizing gas, such as air, for the productionof metal oxide particles. According to other embodiments, the gas supplysystem may provide inert gas such as nitrogen, for the production ofsolid metal particles. Other components not depicted may be used toprovide a suitable ratio of oxidizing to inert gas in the gas supplysystem 270, these components may be pressure swing absorbers,electrolyzers, cryogenic nitrogen tanks, cryogenic oxygen tanks,compressed nitrogen tanks, compressed oxygen tanks, chillers,compressors, or any other related air handling equipment. According tosome embodiments, the gas supply system 270 may supply gas at an ambientenvironmental temperature, such as about 25° C. (e.g., 20-35° C.). Inadditional embodiments, the gas supply may be heated, such as to atemperature of from 25° C. to 5000° C., such as from 25° C. to 50° C.,50° C. to 75° C., 75° C. to 100° C., 100° C. to 125° C., 125° C. to 150°C., 150° C. to 200° C., 200° C. to 250° C., 250° C. to 300° C., 300° C.to 350° C., 350° C. to 400° C., 400° C. to 450° C., 450° C. to 500° C.,500° C. to 550° C., 550° C. to 600° C., 600° C. to 650° C., 650° C. to700° C., 700° C. to 750° C., 750° C. to 800° C., 800° C. to 850° C.,850° C. to 900° C., 900° C. to 950° C., 950° C. to 1000° C., 1000° C. to1100° C., 1100° C. to 1200° C., 1200° C. to 1300° C., 1300° C. to 1400°C., 1400° C. to 1500° C., 1500° C. to 1600° C., 1600° C. to 1700° C.,1700° C. to 1800° C., 1800° C. to 1900° C., 1900° C. to 2000° C., 2000°C. to 2250° C., 2250° C. to 2500° C., 2500° C. to 2750° C., 2750° C. to3000° C., 3000° C. to 3275° C., 3275° C. to 3500° C., 3500° C. to 3750°C., 3750° C. to 4000° C., 4000° C. to 4275° C., 4275° C. to 4500° C.,4500° C. to 4750° C., 4750° C. to 5000° C., or any combination thereof.Other components not depicted may be used to provide process heat to thegas supply system 270, these components may include resistive heaters,heat exchangers, natural gas heaters, boilers, direct combustionheaters, arc heaters, induction heaters, microwave heaters, or any otherrelated process heat systems.

The reaction zone 220 may generally be where the reaction or physicalchange to the molten material takes place. As described herein, the“reaction” may include any chemical or physical change of the injectedmolten metal-containing material. For example, the moltenmetal-containing material may be oxidized in the reaction zone 220.However, in other embodiments, the molten metal-containing material maynot undergo a chemical reaction, and may instead be converted to solidparticles of a similar or smaller size than the molten metal-containingmaterial entering the reaction zone 220. For example, an oxidationreaction may take place when an oxidizing gas, such air, is injectedinto the reaction zone 220. However, nitrogen or other non-reactivegasses may be utilized when oxidation is not desired.

The process may operate at relatively high temperatures, substantiallyabove the melting point of lead which is (621° F.) when oxidized lead isdesired or substantially below the melting point of lead which is 327°C. (620° F.) when powdered lead metal is desired.

Downstream of the reaction vessel may be a separation zone 202. Theseparation zone 202 may include a one or more exhaust ports 215 and oneor more solid particle exits, such as the depicted solid particleremoval pathway 216.

The separation zone may include an upper exhaust region 212 and a lowerfrustum 211. The metal containing particles 219 may accumulate in theseparation zone 202 and be directed to the solid particle removalpathway 216. The solid particle removal pathway 216 may comprise a oneor more of bins, hoppers, chutes, feeders, pneumatic conveyors, beltconveyors, hydraulic conveyors, or any other solid particle transferequipment. Between the reaction zone 220 and / or the separation zone202, it may be necessary to cool the metal containing particles 219.According to some embodiments, a cooling gas or liquid may introduced tothe falling metal containing particles using a cooling air supply 285.The cooling air supply may include a blower 281, an air intake 283, andan air injector 282.

The metal-containing material outlet may comprise, for example a duct,chute, or other passage. The gas may pass into the reaction zone 220 viareaction gas injector 274 and may pass out of the reaction zone (alongwith the solid particle products) via an opening at the bottom of thereaction zone 220. The gas exiting through the bottom of the reactionzone frustum may at least partially aid in transporting the solidparticles out of the reaction zone 220.

The reactor system 200 may additionally include a water inlet (notshown). Water may be injected into the reaction zone 220 to control thetemperature in the reaction zone.

FIG. 4 is a top down perspective view of the reactor system 200, showingthe upper cylindrical section 223 positioned within the upper exhaustregion 212. The housing also contains the one or more exhaust ports 215.According to some embodiments the gas outlets may be round, according toother embodiments they may be square, constitute an annulus surroundingthe upper cylindrical section 223, or be any other shape founddesirable. According to some embodiments the reaction gas injector 274may tangential to the upper cylindrical section 223, such as to causethe molten material and gas to swirl within the reactor, creatingturbulent conditions.

It should be understood that while FIGS. 3 and 4 depict one embodimentof a reactor suitable for the presently described processes, otherreactor configurations are contemplated, such as reactor configurationswith varying geometric shapes and positions for the one or more inletsand outlets of the reactor. For example, the molten material injectordevice 300 may be positioned on the upper cylindrical section 223 of thereactor system 200.

It should be appreciated that a wide variety of injector devices 300 maybe utilized in the disclosed systems and methods, these injector devicesvarying in size, interior shape, etc. According to one or moreembodiments, the molten material injector device 300 may comprise asingle-conduit injector 140. For example, embodiments of single-conduitinjectors are depicted in FIGS. 6, 7A and 7B. As described herein, thesingle-conduit injector 140 may function as an atomizer, or at leastinject molten metal-containing material with a laminar flow. Inadditional embodiments, such as that depicted in FIG. 6, thesingle-conduit injector 140 may include a gas annulus 135 which mayfunction to impinge the flow of the molten metal.

Referring now to FIG. 5, a cross-sectional view of an embodiment of amolten material injector device 300 is depicted. The molten materialinjector device 300 may be comprised of two or more components includinga single-conduit injector 140, depicted in greater detail in at leastFIGS. 6, 7A and 7B, and a gas manifold 130, depicted in greater detailin FIGS. 6 and 9. It should be understood that the single-conduitinjector 140, under certain conditions, may be capable of sufficientlyatomizing the molten metal-containing material without the gas manifold130.

According to one or more embodiments disclosed herein, the moltenmaterial injector device 300 may comprise a single-conduit injector 140,such as depicted in FIG. 5. The single-conduit injector 140 may comprisea cylindrical conduit tube 143 with defined length and inside diameter,with multiple or single inlets 142 located at the molten material feedend 144, and a nozzle 148, with defined geometry and ejection openinglocated at the outlet end 146. Molten materials at variable pressuresmay be introduced into the feed end 144 of single-conduit injector 140and may exit the outlet end 146 in the physical form of a laminar sheetor atomized droplets. A single-conduit injector may improve control ofmolten material atomization, resulting in some embodiments in improvedcontrol of the product particle size distribution, improved control ofresidual free lead, and/or increased lead oxide production rates (inprocesses where lead is oxidized).

As described herein, the molten material injector device 300 mayfunction as an atomizer, or at least inject molten metal-containingmaterial with a laminar flow. In additional embodiments, such as thatdepicted in FIG. 4, the molten material injector device 300 may includea gas annulus 135 which may function to impinge the flow of the moltenmetal.

Various physical parameters characteristic to molten materials (e.g.,molten lead) such as, but not limited to, density viscosity and surfacetension may affect the fluid properties of the molten feed streamexiting the single-conduit injector 140. Various design parameters, suchas, but not limited to injector inlet geometry, injector inlet area,injector inlet perpendicular to tangential orientation, injector insidecylindrical length, injector inside cylindrical diameter, nozzleconverging section design, nozzle throat diameter, and inside surfacefinish may affect the interaction between the molten feed stream and theSingle-Conduit Injector, wherein the control of each of thesecharacteristics are contemplated herein.'

While the reactor systems 100, 200 of FIGS. 1 and 3 depict a singlemolten material injector device 300 positioned at the cover top 106, 206of the reactor 101, 201, it is contemplated that more than one moltenmaterial injector devices 300 may be utilized on a single reactor 101,201 which may be positioned at other areas of the reactor 101, 201. Forexample, molten material injector devices 300 may be positioned on otherportions of the top cover 106, 206 or on the sidewalls 104, 204 of thereactor 101, 201.

As depicted in FIG. 6, in some embodiments the single-conduit injector140 may be positioned to release molten metal-containing material withina gas annulus 135 discharged through gas manifold 130. The gas annulus135 may be supplied by a gas manifold 130 and through a gas discharge133. The gas manifold 130 may be in direct contact with the exterior ofthe single-conduit injector 140. Each of the single-conduit injector 140and the gas manifold 130 may each be assembled from more than one body.For example, in one embodiment, the single-conduit injector device mayhave a lower nozzle piece and an upper cap piece, the two piecesthreading into one another. Other methods of connecting the two piecesare contemplated as well including press fit, adhesives, epoxies,welding, brazing, bolts, external clamps or fittings, and the like.

As depicted in FIG. 6, in one or more embodiments, the moltenmetal-containing material may be dispensed in a hollow conical pattern,which may be contacted by the gas annulus flowing down at a differentangle, such as normal with respect to the top cover 106, 206 of thereactor 101, 201. According to additional embodiments, the moltenmetal-containing material may be atomized by the single-conduit injector140, such as when the single-conduit injector 140 acts as a sprayer.Without being bound by theory, it is believed that when a stream of highviscosity molten metal-containing material, such as lead, flows throughan single-conduit injector 140 at relatively high mass flow rates, thedifference in velocity between the stream of molten metal-containingmaterial and surrounding air, or an inert gas, promote dropletatomization. The atomized droplets may then be introduced into, forexample, the reaction zone 120, 220 of the reactors of FIG. 1 or 3,which may enhance chemical reaction rates and manufacturing output.

According to one or more embodiments, the single-conduit injector 140may produce a laminar flow of molten metal-containing material enteringthe reactor 101, 201 and subsequently the laminar flow may be impingedupon with a high velocity gas annulus 135, as depicted in FIG. 6.Without being bound by theory, it is believed that when streams of highviscosity molten metal-containing materials, such as lead, flow throughan injector, such as the single-conduit injector 140, at relatively lowmass flow rates and are impinged with high velocity gas, atomized moltendroplets may form. The high velocity gas flow may enhance molten leadatomization as the laminar flow of molten lead comes in contact with gasannulus high velocity gas, along with the turbulent gas environment ofthe reactor 101, 201.

According to one or more additional embodiments disclosed herein, themolten material injector device 300 may comprise air sprayers, inert gassprayers, oxidizing gas sprayers, pressure sprayers, electrostaticsprayers, or ultrasonic sprayers. The selection of an appropriate moltenmaterial injector device may affect various properties of the outputproduct material. For example, and without limitation, the injection ofthe molten metal-containing material may be selected to influence one ormore of particle size distribution (lead oxide or free lead), particleshape, lead oxide surface area, lead oxide acid absorption, and/ormanufacturing rate. A desired molten material injector device may alsobe determined by process specification such as head pressure, etc.

Referring now to FIG. 5, a cross-sectional view of an embodiment of amolten material injector device 300 is depicted. The molten materialinjector device may be comprised of two or more components including amolten material injector device 300, depicted in greater detail in FIG.6, and a gas manifold 130, depicted in greater detail in FIG. 7A. Itshould be understood that the molten material injector device 300, undercertain conditions, may be capable of sufficiently atomizing the moltenmetal-containing material without the gas manifold 130. As depicted inFIG. 6, in some embodiments the molten material injector device 300 maybe positioned to release molten metal-containing material within a gasannulus 135 discharged through gas manifold 130. The gas annulus 135 maybe supplied by a gas manifold 130 and through a gas discharge 133. Thegas manifold 130 may be in direct contact with the exterior of themolten material injector device 300. Both the molten material injectordevice 300 and the gas manifold 130 may each be assembled from more thanone body. For example, in one embodiment, the single-conduit injectordevice may have a lower nozzle piece and an upper cap piece, the twopieces threading into one another. Other methods of connecting the twopieces are contemplated as well including press fit, adhesives, epoxies,welding, brazing, bolts, external clamps or fittings, and the like.

Now referring to FIG. 7A, a single-conduit injector 140 is depicted. Thesingle-conduit injector 140 may comprise an outer surface 145; acylindrical conduit tube 143 with defined length and inside diameter;multiple or single inlets 142 located at the molten material feed end144; a converging section 141 with defined length; and a nozzle 149 withdefined length, geometry, and orifice area located at the outlet end146. In some embodiments, such as that as depicted in FIG. 8 themultiple or single inlets 142 may be positioned tangentially to thecircumference of the cylindrical conduit tube 143, and normal to theheight of the conduit tube. The top 144 of the single-conduit injector140 may be circular and cap the device.

According the some embodiments, the angle between converging section 141and the cylindrical conduit tube 143 may be from 90° to 180°, such asfrom 90° to 115°, from 115° to 130°, from 130° to 145°, from 145° to160°, from 160° to 175°, from 175° to 180°, or any combination thereof.

It should be appreciated that one or more embodiments of the disclosedsingle-conduit injector 140 may not include a converging section 141(e.g. ,the cylindrical conduit tube 143 has a diameter about the same asthe nozzle 149. This can be considered analogous to the angle betweenthe converging section 141 and the cylindrical conduit tube 143 equal toabout 180° (i.e., on the same plane).

As depicted in FIG. 6, molten metal-containing material may enter thesingle-conduit injector at the one or more inlets 142, travel throughthe converging section 141 towards the nozzle 149. As the moltenmetal-containing material travels across the converging section theavailable cross sectional area decreases and the speed of the materialincreases. The parameters which control the eventual mass and velocityof the molten metal-containing material as it exits the outlet end 146are the inlet pressure, inlet 142 diameter and position, the cylindricalconduit tube 143 length and diameter, the converging section 141 lengthand angle, and the nozzle 149 length and diameter. In some embodimentsthe configuration of the single-conduit injector will cause the moltenmetal-containing material to spray out in a hollow cone, in otherembodiments the molten metal-containing material may spray out in otherpatterns such as a swirl or a stream.

As depicted in FIG. 8, in one or more embodiments, as the moltenmetal-containing material enters the single-conduit injector 140 throughthe one or more inlets 142, it swirls within the cylindrical conduittube 143. This further affects the flow profile of the moltenmetal-containing material as it exits through the nozzle 149.

As depicted in FIG. 6, the single-conduit injector 140 may be positionedin the center of a gas annulus 135 with defined diameter and gap width.Molten metal-containing materials at variable pressures may beintroduced into the feed end 144 of single-conduit injector 140 and mayexit the outlet end 146 in the physical form of a laminar sheet oratomized droplets. A high velocity flow of gas 135 (in an annulus)impinges upon the laminar flow of molten lead such that atomization ofmolten metal-containing material is enhanced, resulting in someembodiments in improved control of the product particle sizedistribution, improved control of residual free lead, and/or increasedlead oxide production rates (in processes where lead is oxidized.

Referring now to FIG. 9, a bottom up view of a gas manifold 130 isdepicted. In some embodiments, one or more gas supplies 132 enter fromthe side of a spherical manifold. According to other embodiments theexterior of the manifold may be square, rectangular, octagonal, or anyother geometric shape. In embodiments which utilize the gas manifold,the single-conduit injector 140 passes molten metal-containing materialthrough a molten metal material injector opening 134. The single-conduitinjector may be disposed within a molten metal material injector opening134 or it may be disposed above the opening and release moltenmetal-containing material through the opening. In some embodiments, gasenters through the one or more gas supplies 132 and exits through thegas discharge 133, preferably, substantially all of the gas exitsperpendicular to the diameter of the cylindrical conduit tube 143. Thisgas exiting the gas discharge 133 forms the gas annulus 135 inembodiments which utilize a gas annulus. A molten metal materialinjector opening 134 may comprise an inner diameter and an outerdiameter. The inner diameter of the gas discharge may be from 3 to 10in, or from 5 to 9 in, or from 6 to 8 in. The outer diameter of the gasdischarge may be from 0.0001 in to 2 in, or from 0.0005 in to 1 in, orfrom 0.001 in to 0.1 in, or from 0.001 in to 0.01 in, larger than theinner diameter of the gas discharge.

According to one or more embodiments, the molten material injectordevice 300 may atomize the molten metal-containing material to a d₅₀size of from 1 to 5 microns, from 5 microns to 10 microns, from 10microns to 25 microns, from 25 microns to 50 microns, from 50 microns to100 microns, from 100 microns to 150 microns, from 150 microns to 200microns, from 200 microns to 250 microns, from 250 microns to 300microns, or any combination thereof. The atomized introduction of moltenmetal to the reactor 101 may result in solid product particles having ad₅₀ of from 0.5 microns to 300 microns (such as from 0.5 microns to 5microns, from 5 microns to 10 microns, from 10 microns to 25 microns,from 25 microns to 50 microns, from 50 microns to 100 microns, from 100microns to 200 microns, from 200 microns to 300 microns, or anycombination thereof. The product particles may have a relatively uniformsize.

According to one or more embodiments, the molten material injectordevice 300 may produce a laminar flow of molten metal-containingmaterial entering the reactor 101, 201. Without being bound by theory,it is believed that when streams of high viscosity moltenmetal-containing materials, such as lead, flow through an moltenmaterial injector device 300 at relatively low mass flow rates, absentof any external gas turbulence, molten droplets may form and align inparallel streams resulting in a laminar flow. The laminar flow may be aparabolic stream in appearance and may enhance molten lead atomizationas the laminar flow enters the turbulent environment of the reactor 101,201.

According to one or more embodiments, the velocity, temperature,viscosity, density, and/or surface tension of the moltenmetal-containing material feed stream may influence the atomizationproperties, such as droplet size. In some embodiments, the molten streamvelocity entering the reactor 101, 201 may be increased by controllingthe molten metal-containing material stream head pressure, such that themass flow rate exceeds the mass flow rate feed typical of a standardBarton Reactor. The relatively high pressure may also result in reducedmolten particle size (i.e., increased atomization).

In one or more embodiments, the reactor system 100, 200 fitted with amolten material injector device 300 may be capable atomizing a moltenstream of lead into solid particles that are significantly smaller thandroplet sizes achieved by a traditional Barton Reactor (i.e., one inwhich molten metal-containing material enters in a non-atomized form).Therefore, the presently described reactor systems may be capable ofhigher production rates when compared to conventional Barton technology.

While the reactor systems 100, 200 of FIGS. 1 and 3 depict a singlemolten material injector device 300 positioned at the cover top 106, 206of reactor 101, 201 it is contemplated that more than one moltenmaterial injector devices 300 may be utilized on a reactor 101, 201,which may be positioned at other areas of the reactor 101, 201. Forexample, molten material injector devices 300 may be positioned on otherportions of the vessel top 106, 206 or on the sidewalls 104, 204 of thereactor 101, 201.

Various physical parameters characteristic to molten metal-containingmaterials (e.g., molten lead) such as, but not limited to, densityviscosity and surface tension may affect the fluid properties of themolten feed stream exiting the single-conduit injector 140. Variousdesign parameters, such as, but not limited to injector inlet geometry,injector inlet area, injector inlet perpendicular to tangentialorientation, injector inside cylindrical length, injector insidecylindrical diameter, nozzle converging section design, nozzle throatdiameter, and inside surface finish may affect the interaction betweenthe molten feed stream and the Single-Conduit Injector, wherein thecontrol of each of these characteristics are contemplated herein.

In additional embodiments, various operating parameters relative to themolten metal-containing material (such as metallic lead) such as, butnot limited to, temperature, mass flow rate, head pressure, and/orsuperficial velocity, may affect the interaction between the molten feedstream and the single-conduit injector 140, such that the molten leadexiting the nozzle 149 of the single-conduit injector 140 efficientlyand/or controllably forms a laminar sheet, a stream of atomizeddroplets, or a uniform diameter flow.

According to one or more embodiments, the temperature of a moltenmetal-containing material feed stream entering the single-conduitinjector 140 may be controlled to attain a desired moltenmetal-containing material density, viscosity, and/or lead surfacetension, such that the desired atomization and droplet size areachieved. For example, molten lead may be at a temperature greater thanlead's melting point, 327.5° C., and less than lead's boiling point,1,740° C., such that the molten lead density is conducive to achieve thedesired laminar flow, atomization and/or droplet size.

According to one or more embodiments, the superficial velocity, headpressure, of a molten metal-containing material feed stream within thesingle-conduit injector 140 may be controlled to attain a desiredlaminar flow or atomized droplet size. For example, the laminar velocitymay be from 1 m/s to 100 m/s. The head pressure may be from 1 psi to 250psi. In one or more embodiments, superficial velocity, mass flow rate,head pressure, and/or the free material's reactivity with oxygen may befunctions of the temperature of the molten metal-containing materialfeed stream entering and exiting the single-conduit injector 140. Forexample, if lead is processed, the temperature of the molten lead may befrom 327.5° C. to 1740° C. According to one or more embodiments, themass flow rate of the molten lead into the reactor 101, 201 maydetermine the process production rate of product solid particles. In oneor more embodiments, mass flow rates are attainable from 500 lb/hr to20,000 lb/hr.

Referring again to FIG. 7A, according to some embodiments, the inlet 142diameter could be from 0.01 in to 1 in, or from 0.03 in to 0.16 in, orfrom 0.03 in to 0.125 in, or from 0.089 in to 0.125 in. The discharge146 diameter could be from 0.1 in to 1 in, or from 0.25 in to 1.6 in, orfrom 0.35 in to 0.55 in. The outlet end 146 length could be from 0.1 into 2 in, or from 0.1 in to 1 in or from 0.25 in to 0.5 in. The length ofthe converging section could be 0 in, or from 0.1 in to 1 in, or from0.25 in to 1 in, or from 0.25 in to 0.5 in. The conduit tube 143diameter could be from 0.1 in to 8 in, or from 0.2 in to 6 in, or from0.25 in to 2 in, or from 0.5 in to 1.5 in. The cylindrical conduit tube143 length could be from 0.1 in to 8 in, or from 0.25 in to 6 in, orfrom 0.5 in to 4 in, or from 2 in to 4 in. The single-conduit injector140 may be constructed of metal and may be polished to a 300 grit finishin its interior.

Referring now to FIG. 7B, according to some embodiments, the inlet 142diameter may be substantially aligned with the cylindrical conduit tube143. The converging section 141 may be substantially perpendicular tothe cylindrical conduit tube 143. Single-conduit injector 140 may beconfigured with a variety of attachment mechanisms including threads,glue, welding, epoxy, brazing, or press fittings. According to oneembodiment, outer surface 145 includes threads. Inlet 142 diameter maybe from 0.1 in to 1 in, such as, from 0.1 in to 0.2 in, or from 0.2 into 0.3 in, or 0.3 in to 0.4 in, or from 0.4 in to 0.5 in, or from 0.5 into 0.6 in, or from 0.6 in to 0.7 in, or from 0.7 in to 0.8 in, or from0.8 in to 0.9 in, or from 0.9 in to 1 in, or any combination thereof.The discharge 146 diameter may be from 0.05 in to 0.3 in, such as from0.05 in to 0.06 in, or from 0.06 in to 0.07 in, or from 0.07 in to 0.08in, or from 0.08 in to 0.09 in, or from 0.09 in to 0.1 in, or from 0.1in to 0.11 in, or from 0.11 in to 0.12 in, or from 0.12 in to 0.13 in,or from 0.13 in to 0.14 in, or from 0.14 in to 0.15 in, or from 0.15 into 0.16 in, or from 0.16 in to 0.17 in, or from 0.17 in to 0.18 in, orfrom 0.18 in to 0.19 in, or from 0.19 in to 0.20 in, or from 0.20 in to0.21 in, or from 0.21 in to 0.22 in, or from 0.22 in to 0.23 in, or from0.23 in to 0.24 in, or from 0.24 in to 0.25 in, or from 0.25 in to 0.26in, or from 0.26 in to 0.27 in, or from 0.27 in to 0.28 in, or from 0.28in to 0.29 in, or from 0.29 in to 0.30 in, or any combination thereof.According to some embodiments, the single-conduit injector 140 may becomprised of steel, or stainless steel, or iron, or nickel, or titanium,or copper, or brass, or ceramic, or glass, or a combination thereof.

Referring again to FIG. 7A, according to some embodiments, the inlet 142diameter could be from 0.01 in to 1 in, or from 0.03 in to 0.16 in, orfrom 0.03 in to 0.125 in, or from 0.089 in to 0.125 in. The discharge146 diameter could be from 0.1 in to 1 in, or from 0.25 in to 1.6 in, orfrom 0.35 in to 0.55 in. The oulet end 146 length could be from 0.1 into 2 in, or from 0.1 in to 1 in or from 0.25 in to 0.5 in. The length ofthe converging section could be 0 in, or from 0.1 in to 1 in, or from0.25 in to 1 in, or from 0.25 in to 0.5 in. The conduit tube 143diameter could be from 0.1 in to 8 in, or from 0.2 in to 6 in, or from0.25 in to 2 in, or from 0.5 in to 1.5 in. The cylindrical conduit tube143 length could be from 0.1 in to 8 in, or from 0.25 in to 6 in, orfrom 0.5 in to 4 in, or from 2 in to 4 in. The single-conduit injector140 may be constructed of metal and may be polished to a 300 grit finishin its interior.

According to one or more embodiments described herein, lead may bemelted and fed to the reactor, where at least a portion of the lead isoxidized by an oxidizing gas, into lead oxide. The oxidation reactionmay be exothermic and produce different lead oxide morphologiesdepending upon reaction conditions. For example, alpha (tetragonal) leadoxide may be formed, which may be brown or red in color, and beta(orthorhombic) lead oxide may be formed, which may be green to yellow incolor. Some lead may not be oxidized, referred to as free lead. Thephysical properties of the products may be customized based on processinputs.

In one or more embodiments, the product material of the presentlydescribed processes may comprise from 0 wt. % to 100 wt. % oforthorhombic lead monoxide. For example, the product material maycomprise orthorhombic lead monoxide in an amount of from 0 wt. % to 10wt. %, from 10 wt. % to 20 wt. %, from 20 wt. % to 30 wt. %, from 30 wt.% to 40 wt. %, from 40 wt. % to 50 wt. %, from 50 wt. % to 60 wt. %,from 60 wt. % to 70 wt. %, from 70 wt. % to 80 wt. %, from 80 wt. % to90 wt. %, from 90 wt. % to 100 wt. %, or any combination thereof.

In additional embodiments, the product material of the presentlydescribed processes may comprise from 0 wt. % to 100 wt. % of tetragonallead monoxide. For example, the product material may comprise tetragonallead monoxide in an amount of from 0 wt. % to 10 wt. %, from 10 wt. % to20 wt. %, from 20 wt. % to 30 wt. %, from 30 wt. % to 40 wt. %, from 40wt. % to 50 wt. %, from 50 wt. % to 60 wt. %, from 60 wt. % to 70 wt. %,from 70 wt. % to 80 wt. %, from 80 wt. % to 90 wt. %, from 90 wt. % to100 wt. %, or any combination thereof.

According to additional embodiments, the product material of thepresently described processes may comprise from 0 wt. % to 100 wt. % ofmetallic lead (sometimes referred to as powdered lead or free lead whenlead oxide is produced). For example, the product material may comprisemetallic lead in an amount of from 0 wt. % to 10 wt. %, from 10 wt. % to20 wt. %, from 20 wt. % to 30 wt. %, from 30 wt. % to 40 wt. %, from 40wt. % to 50 wt. %, from 50 wt. % to 60 wt. %, from 60 wt. % to 70 wt. %,from 70 wt. % to 80 wt. %, from 80 wt. % to 90 wt. %, from 90 wt. % to100 wt. %, or any combination thereof. The metallic lead may comprise atleast 99 wt. %, 99.5 wt. %, 99.9 wt. %, or even 99.99 wt. % of a lead.

According to additional embodiments, the product material of thepresently described processes may comprise a mixture of tetragonal leadmonoxide, orthorhombic lead monoxide and metallic lead (otherwisereferred to as free lead), in all proportions from 0 wt. % to 100 wt.for any single component. Typical requirements for lead acid batteryactive material specify a mixture of tetragonal lead monoxide as a majorcomponent, metallic lead as a minor component and orthorhombic leadmonoxide permissible in small amounts. For example, the product maycomprise of a mixture of tetragonal lead monoxide, orthorhombic leadmonoxide and metallic lead in the wt. % proportions of: 90:0:10,85:0:15, 80:0:20, 75:0:25, 70:0:30, 65:0:35, 90:5:5, 85:5:10, 80:5:15,75:5:20, 70:5:25, 65:5:30, 60:5:35, 80:15:5, 75:15:10, 70:15:15,65:15:20, 60:15:25, 55:15:30, 50:15:35, or in any other 3-componentcombination thereof. However, some lead acid battery technologies mayrequire a mixture with a greater portion of orthorhombic lead monoxide.For example, the product may comprise of a mixture of tetragonal leadmonoxide, orthorhombic lead monoxide and metallic lead, where theorthorhombic portion may comprise in an amount from 15 wt. % to 20 wt.%, 20 wt. % to 25 wt. %, 25 wt. % to 30 wt. %, 30 wt. % to 35 wt. %, 35wt. % to 40 wt. %, 40 wt. % to 45 wt. %, 45 wt. % to 50 wt. %, or anycombination thereof.

According to additional embodiments, the product material of thepresently described processes may comprise from 0 wt. % to 100 wt. % oflead monoxide. For example, the product material may comprise lead oxidein an amount of from 0 wt. % to 10 wt. %, from 10 wt. % to 20 wt. %,from 20 wt. % to 30 wt. %, from 30 wt. % to 40 wt. %, from 40 wt. % to50 wt. %, from 50 wt. % to 60 wt. %, from 60 wt. % to 70 wt. %, from 70wt. % to 80 wt. %, from 80 wt. % to 90 wt. %, from 90 wt. % to 100 wt.%, or any combination thereof.

According to additional embodiments, the product material of thepresently described processes may comprise BET surface area of from 0.1m²/g to 3.0 m²/g.

According to additional embodiments, the product material of thepresently described processes may have acid absorption of from 100 mgH₂SO₄/g PbO to 300 H₂SO₄/g PbO, such as 140 H₂SO₄/g PbO to 260 H₂SO₄/gPbO.

It has been discovered that the introduction of a moltenmetal-containing material into a molten material injector device 300using a molten material pump 165 may induce variation in mass flow rateand head pressure, leading to variation in the size and quality of metalor metal oxide particles produced in a reactor. As such, in one or moreembodiments, as depicted in FIGS. 5 and 10, molten material reservoir isutilized to control the head pressure of the molten metal-containingmaterial. The molten metal-containing material may pass through areservoir 161 before entering the molten material injector device 300.The reservoir 161 may comprise a pipe or other vessel. For example, thereservoir 161 may comprise a pipe having an internal size of 6.00 to 12inches in diameter and a length of from 1 to 600 inches. The top of thereservoir 161 may be open to the atmosphere, while the bottom may becapped with a base 174. The center of the base 174 may be drilled andthreaded to a diameter and thread size appropriate to receive thethreaded single-conduit injector 140, as shown in FIG. 5. Thesingle-conduit injector may be threaded into the base 174 of thereservoir 161 such that the inlets 142 of the single-conduit injector140 are centered and, for example, 0.05 to 1.0 inches from the base 174.

The reservoir 161 may be heated to prevent the molten metal-containingmaterial from freezing. The reservoir pipe may be enclosed with aninsulated (e.g., 12-inch) duct with a hot gas inlet 180 located at thebase and hot gas outlet 182 located at the top of the duct, opposite ofthe hot gas inlet 180. A molten material supply pipe 184 may extendthrough the lower portion of the duct opposite of the hot gas inlet 180and supply molten metal-containing material to the reservoir 161. Themolten material supply pipe 184 may be in fluid communication with themolten metal-containing material source 162, 262 or may be the sameapparatus as the molten metal-containing material source 162, 262 ofFIGS. 1 and 3.

The reservoir 161 may comprise a head pressure gauge 190, which may beutilized to measure the pressure of the molten metal-containing materialat the inlet 142 of the molten material injector device 300.Additionally, a molten material volume monitor 150 (such as a moltenmaterial height or level monitor) is also utilized in the reservoir 161to measure the height of the molten metal-containing material in thereservoir. The reservoir may be utilized to keep head pressurerelatively constant by maintaining a relatively constant amount ofmolten metal-containing material in the reservoir (i.e., a relativelyconstant height of molten metal-containing material). For example, therate or introduction of molten metal-containing material into thereaction zone 108 may not vary by more than 20%, more than 10%, morethan 5%, or even by more than 1%.

The molten material volume monitor 150 may comprise any device operableto monitor the height of the molten metal-containing material in thereservoir 161. For example, and without limitation, pressure gaugesand/or visual monitors may be utilized to monitor the height. The amountof molten metal-containing material in the reservoir 161 is thenmanipulated by adding additional molten metal into the reservoir 161 viamolten material supply pipe 184. Suitable pressure gauges may include,without limitation, manometers, analog, or digital pressure gauges,LASER implemented monitoring devices, cameras, sonic or sonar devices,or piezo-electric devices.

According to one or more embodiments, a method for processing moltenmetal-containing materials into particles may include monitoring orsetting a target head pressure for the molten material injector 140 byutilizing the head pressure gauge 190. For example, if a known headpressure is desired, the head pressure gauge 190 can be utilized todetermine the approximate height of molten metal in the reservoir 161that will produce such a head pressure. Thereafter, the target headpressure may be held by utilizing the molten material volume monitor 150(such as a manometer) to control when and how much additional moltenmetal-containing material is passed into the reservoir 161. Thus, theheight of material in the reservoir may be relatively constant, causingthe head pressure to be relatively constant.

For example, according to at least one embodiment, the molten materialvolume monitor 150 in conjunction with the valve 164 controlling flowrate of molten metal-containing material, may maintain the molten flowinto the reactor 101, 201 within 1% or even within 0.1%. A ReliablePressure Drop Device such as a valve, orifice, atomizer, injector,nozzle or any other suitable device may be used to generate a repeatablepressure difference.

According to one or more embodiments, the molten material volume monitor150 may comprise a manometer 152, such as shown in FIG. 5. The preciselevel of molten material can be maintained in the reservoir 161 byutilizing the difference in densities of the molten material, such aslead, and water. A manometer 152 calibrated in 1/10's of an inch ofwater column is inserted in the reservoir 161. A bleed valve 154 may beinserted in the tube 156 between the reservoir 161 and the water 158 inthe manometer 152. The bleed valve 154 is initially left open toatmosphere. When the desired level of molten material has been reachedin the reservoir 161, as measured on the head pressure gauge 190, thebleed valve 154 is closed. After the bleed valve 154 is closed,variations in the level in the reservoir 161 register a change in theheight of the water 158 in the manometer. An electronic controller maymonitor the manometer 152 and send a signal to open or close the valve164 (increasing or decreasing mass flow rate of molten material throughthe molten material supply pipe 184).

For example, the density of lead is about 11 times that of water.Therefore, a 0.01 inch change in lead level results in 0.11 inch changeon a gauge measuring in inches of water. The density effect magnifiessmall changes in lead levels into larger changes in water levels. Themore sensitive manometer 152 is used to control the lead level in thereservoir 161 by sending a signal to the valve 164 attached to the meltkettle to maintain proper molten lead level in the reservoir.

According to one or more embodiments, the velocity, temperature,viscosity, density, and/or surface tension of the molten material feedstream may influence the atomization properties, such as droplet size.In some embodiments, the molten stream velocity entering the reactor101, 201 may be increased by controlling the molten material stream headpressure, such that the mass flow rate exceeds the mass flow rate feedtypical of a standard Barton Reactor. The relatively high pressure mayalso result in reduced molten particle size (i.e., increasedatomization).

In one or more embodiments, a Barton reactor fitted with asingle-conduit injector 140 may be capable atomizing a molten stream oflead into solid particles that are significantly smaller than dropletsizes achieved by a traditional Barton Reactor (i.e., one in whichmolten material enters in a non-atomized form). Therefore, a Bartonreactor fitted with a single-conduit injector 140 may be capable ofhigher production rates when compared to conventional Barton technology.

Now referring to FIG. 11, another system suitable for the formation ofmetallic or metal oxide powders is disclosed. According to one or moreembodiments, a feed stream may be passed through a first conduit of themulti-conduit reactor, and a fluid stream may be passed through a secondconduit of the multi-conduit reactor, where the feed stream and thefluid stream contact one another in a mixing zone and form a productstream which exits the multi-conduit reactor. Optionally, a quenchstream may further enter the mixing zone through a third conduit.Various process parameters such as, but not limited to, streamcompositions, stream temperatures, stream flow rates, and streamsuperficial velocities may affect the interaction between the feedstream and the fluid stream.

Referring to FIG. 11, a multi-conduit reactor 800 is schematicallydepicted. The multi-conduit reactor 800 may comprise at least a firstconduit 810 and a second conduit 830 which lead to a mixing zone 870.The first conduit 810 may include an inlet 812 and an outlet 814, andthe second conduit 830 may include an inlet 832 and an outlet 834. Thefirst conduit 810 and the second conduit 830 may be divided from oneanother by a first tubular wall 816. As depicted in FIG. 11, the firstconduit 810 and the second conduit 830 may form a coaxial geometry, suchthat the first conduit 810 is axially surrounded by the second conduit830. The second conduit 830 may be defined by the first tubular wall 816on its inner perimeter and by a second tubular wall 836 on its outerperimeter. According to some embodiments, the multi-conduit reactor 800may additionally comprise a third conduit 850 defined by the secondtubular wall 836 and a third tubular wall 856. The first conduit 810,the second conduit 830, and the third conduit 850 may form a multi-axialgeometry where the second conduit 830 axially surrounds the firstconduit 810 and the third conduit 850 axially surrounds the secondconduit 830.

According to some embodiments, at least a portion of the first tubularwall 816 may be circular in cross-section, such as the embodimentschematically depicted in FIG. 12. In such an embodiment, at least aportion of the first conduit may have a circular cross-section definedby the first tubular wall 816 as its outer perimeter. In someembodiments, the second tubular wall 836 may be circular incross-section. In such an embodiment, at least a portion of the secondconduit 830 may have a circular inner cross section and a circular outercross section (i.e., ring shaped). At least a portion of the thirdconduit 850 may likewise have a circular inner cross-section and acircular outer cross-section, as depicted in FIG. 12.

According to some embodiments, the entirety of the first conduit may betubular in shape, where a substantially straight pathway connects thefirst conduit inlet 812 and the first conduit outlet 814. The secondconduit 830 may have an annular cross-section surrounding a portion ofthe first conduit, and may have an inlet 832 which emanates from a sideof the multi-conduit reactor 800. In some embodiments, the third conduit850 may also have an annular cross-section and have an inlet 852 whichemanates from a side of the first reactor 800. FIG. 12 schematicallydepicts a top view of the axially aligned first conduit 810, secondconduit 830, and third conduit 850, where the second conduit 830 has itsinlet 832 emanating from a side of the multi-conduit reactor 800, andwhere the third conduit 850 has its inlet 852 emanating from a side ofthe multi-conduit reactor 800.

In one or more embodiments, the first conduit 810 may taper outward ator near its outlet 814, such that its cross-sectional area is greater ator near the outlet 814 than at or near the inlet 812 or area of thefirst conduit 810 between the inlet 812 and the outlet 814. The secondconduit 830 and third conduit 850 may each taper inwards at or neartheir respective outlets 834, 854.

The first conduit 810, the second conduit 830, and the optional thirdconduit 850 may lead into a mixing zone 870, which may be substantiallycylindrical in shape (i.e., having a circular cross-section.) The mixingzone 870 may be defined by a mixing zone wall 872. Product streams mayflow out of the mixing zone 870, and the multi-conduit reactor 800,through the outlet 874.

According to various embodiments, the cross-sectional area of the firstconduit 810 at the outlet 814 may be from 0.049 square inches to 0.45square inches. For example, the cross-sectional area of the firstconduit 810 at the outlet 814 may be from 0.049 square inches to 0.1square inches, from 0.1 square inches to 0.2 square inches, from 0.2square inches to 0.3 square inches, or from 0.3 square inches to 0.4square inches. The first conduit 810 may be tapered such that thecross-sectional area of the first conduit 810 at the outlet 814 isgreater than the cross-sectional area of the first conduit 810 at ornear the inlet 812. For example, the cross-sectional area of the firstconduit 810 at or near the inlet 812 may be from 0.049 square inches to0.2 square inches, such as from 0.049 square inches to 0.1 squareinches, from 0.1 square inches to 0.15 square inches, or from 0.15square inches to 0.2 square inches.

The cross-sectional area of the second conduit 830 at the outlet 834 maybe from 0.49 square inches to 7.1 square inches. For example, thecross-sectional area of the second conduit 830 at the outlet 834 may befrom 0.49 square inches to 2 square inches, from 2 square inches to 4square inches, from 4 square inches to 7.1 square inches, or from 0.5square inches to 1.5 square inches. The second conduit 830 may betapered such that the cross-sectional area of the second conduit 830 atthe outlet 834 is less than the cross-sectional area of the secondconduit 830 at or near the inlet 832. For example, the cross-sectionalarea of the second conduit 830 at or near the inlet 832 may be from 0.78square inches to 7.1 square inches, such as from 0.78 square inches to 2square inches, 2 square inches to 4 square inches, from 4 square inchesto 7.1 square inches, or from 2.5 square inches to 3 square inches.

The cross-sectional area of the third conduit 850 at the outlet 854 maybe from 0.5 square inches to 20 square inches. For example, thecross-sectional area of the first conduit 850 at the outlet 854 may befrom 0.5 square inches to 5 square inches, from 5 square inches to 10square inches, from 10 square inches to 15 square inches, from 15 squareinches to 20 square inches, or from 0.5 square inches to 1.5 squareinches. The third conduit 850 may be tapered such that thecross-sectional area of the third conduit 850 at the outlet 854 is lessthan the cross-sectional area of the third conduit 850 at or near theinlet 852. For example, the cross-sectional area of the third conduit850 at or near the inlet 852 may be from 3 square inches to 20 squareinches, such as from 8 square inches to 9.5 square inches, from 3 squareinches to 7 square inches, from 7 square inches to 14 square inches, orfrom 14 square inches to 20 square inches.

According to one or more embodiments, the ratio of the cross-sectionalarea of the third conduit 850 at the outlet 854 to the cross-sectionalarea of the second conduit 830 at the outlet 834 is from 0 to 3, such asfrom 0 to 1, from 1 to 2, from 2 to 3, or from 0.7 to 1.1.

The various portions of the multi-conduit reactor 800 may be constructedfrom a wide variety of materials which are suitable for the thermalloads required by the methods described herein. For example, one or moreportions of the multi-conduit reactor may be made of Inconel alloy (suchas Iconel 601) or Haynes 230 alloy, which may be capable of withstandingtemperatures of up to 2100° F.

It should be understood that the various streams may be characterized bytheir momentum flux, their superficial velocity, mass flowrate, etc.These properties, unless stated otherwise, are described with relationto the given stream as it enters the mixing zone 870 (i.e., at the feedstream outlet 814, the fluid stream outlet 834, and the quench streamoutlet 854, respectively).

It should be appreciated that the design of the multi-conduit reactor800 may be varied according to embodiments of the presently disclosedmethods for processing metals and alloys disclosed herein. For example,the cross-sectional shape and/or relative size of one or more of thefirst conduit 810, the second conduit 830, and/or the third conduit 870may be different from that depicted in FIG. 11 and described herein. Forexample, the conduits 810, 830, 850 may not share common walls with oneanother, and may have different shapes. Additionally, it should beappreciated that in some embodiments a third conduit 850 may not beincluded in the multi-conduit reactor 800. In additional embodiments,the conduit outlets 814, 834, 854 may be positioned on other portions ofthe mixing zone 870, and may not be adjacent to one another.

Now referring to FIG. 13, a reactor system 900 is depicted whichincludes, in addition to the multi-conduit reactor 800 of FIG. 11,additional stream pre-processing units such as a feed streampre-processing unit 910, a fluid stream pre-processing unit 920, and aquench stream pre-processing unit 930. The pre-processing units 910,920, 930 may change the temperature, pressure, or other characteristicsof a given stream such a mass flow rate or superficial velocity. A feedstream pre-processing unit 910 may treat the feed stream 912 prior tothe feed stream 912 entering the multi-conduit reactor 800. In oneembodiment, the pre-processing unit 910 may heat the feed stream 912 toa temperature which liquefies the metals and/or alloys of the feedstream. In such embodiments, the feed stream pre-processing unit 910 maycomprise a heater or heat exchanger. The fluid stream pre-processingunit 920 may treat the fluid stream 922 prior to the fluid stream 922entering the multi-conduit reactor 800. In one embodiment, the fluidstream pre-processing unit 920 may heat the fluid stream 922 as well aspressurize the fluid stream 922. In such embodiments, the fluid streampre-processing unit 920 may comprise a compressor, pump, or otherpressure altering means, and a heater or heat exchanger. The quenchstream pre-processing unit 930 may treat the quench stream 932 prior tothe quench stream 932 entering the multi-conduit reactor 800. In oneembodiment, the quench stream pre-processing unit 920 may cool thequench stream 932. For example, the quench stream pre-processing unit930 may include a refrigeration means or heat exchanger.

Referring again to FIG. 11, in operation of the multi-conduit reactor800, a feed stream may be passed through the first conduit 810 and afluid stream may be passed through the second conduit 830. The feedstream may be contacted by the fluid stream in the mixing zone 870.Contact of the feed stream with the fluid stream may cause a chemicalchange and/or physical change in the feed stream, producing a productwhich exits the multi-conduit reactor 800 through the mixing zone outlet874 in a product stream. A quench stream may also enter the mixing zone870 via the third conduit 850 and mix with one or more of the feedstream, the fluid stream, or some product formed by the contact betweenthe feed stream and the conduit stream.

In one or more embodiments, the feed stream may comprise one or moremetal compounds, or alloys thereof. Throughout this disclosure, itshould be understood that the term metal may include an alloy. Accordingto one embodiment, the feed stream may comprise one or more metals in anamount of at least 50 wt. % of the total mass of the feed stream. Inadditional embodiments, the feed stream comprises one or more metals inan amount of at least 60 wt. %, at least 70 wt. %, at least 80 wt. %, atleast 90 wt. %, at least 95 wt. %, at least 98 wt. %, or even at least99 wt. % of the total mass of the feed stream. In some embodiments, themetal in the feed stream may consist essentially of, or consists of, asingle metal or alloy species. For example, the metal or alloy in thefeed stream may consist essentially of lead.

The feed stream may additionally include a carrier gas. The carrier gasmay serve to move the feed stream in a direction generally towards themulti-conduit reactor 800 and into the mixing zone 870. In someembodiments, the carrier gas may be an inert gas, such as nitrogen. Inadditional embodiments, the carrier gas may be air or another gas thatincludes oxygen or other reactive species.

The feed stream may be heated to an elevated temperature, such that themetals or alloys of the feed stream are molten. For example, the feedstream may have a temperature greater than or equal to the melting pointof the material of the feed stream. If more than one material iscontained in the feed stream, the melting point of the feed stream maybe considered to be the melting point of the lowest melting pointmaterial in the feed stream or the melting point of the feed stream maybe considered as the eutectic melting point which is a temperature thatis lower than the melting point for any single mixture constituent. Inadditional embodiments, the feed stream may be at a temperature greaterthan or equal to the melting point of the highest melting point materialin the feed stream or greater than the eutectic melting point formixtures comprising multiple molten metals. For example, if lead isprocessed in the multi-conduit reactor 800, the feed stream may have atemperature of at least about 621.5° F., which is the melting point oflead.

According to various embodiments, the feed stream may have a temperatureof at least 50° F., at least 100° F., at least 150° F., at least 200°F., at least 250° F., at least 300° F., at least 350° F., at least 400°F., at least 450° F., at least 500° F., at least 550° F., at least 600°F., at least 650° F., at least 700° F., at least 750° F., at least 800°F., at least 850° F., at least 900° F., at least 950° F., at least 1000°F., at least 1050° F., at least 1100° F., at least 1150° F., at least1200° F., at least 1250° F., at least 1300° F., at least 1350° F., atleast 1400° F., at least 1450° F., or even at least 1500° F. Forexample, the feed stream may have a temperature of from 400° F. to 1200°F., such as from 500° F. to 1000° F., from 600° F. to 800° F., or from650° F. to 750° F. In additional embodiments, the feed stream may have atemperature of at least the melting point of any of the metals or alloysidentified herein or the feed stream may have a eutectic melting pointtemperature of any metal or metalloid mixtures or metal alloys.

The feed stream may have a superficial velocity of from 0.1 ft/s to 100ft/s. For example, the superficial velocity of the feed stream may be atleast 0.1 ft/s, at least 0.5 ft/s, at least 1 ft/s, at least 5 ft/s, atleast 10 ft/s, or at least 30 ft/s, such as from 0.1 ft/s to 1 ft/s,from 1 ft/s to 10 ft/s, from 10 ft/s to 50 ft/s, or from 50 ft/s to 100ft/s.

The feed stream may have a mass flowrate of from 0.2 lbs/s to 10 lbs/s.For example, the mass flowrate of the feed stream may be at least 0.2lbs/s, at least 0.5 lbs/s, at least 1 lbs/s, at least 3 lbs/s, or atleast 5 lbs/s, such as from 0.2 lbs/s to 1 lbs/s, from 1 lbs/s to 3lbs/s, from 3 lbs/s to 5 lbs/s, from 5 lbs/s to 7 lbs/s, or from 7 lbs/sto 10 lbs/s.

The fluid stream may comprise one or more chemical species in a gasphase. According to some embodiments, the fluid stream may comprise acombustible gas, such as oxygen. For example, the fluid stream maycomprise, consist essentially of, or consist of air. In one or moreembodiments, the fluid stream may comprise oxygen in an amount of atleast 5 wt. % of the total mass of the fluid stream. In additionalembodiments, the fluid stream may comprise oxygen in an amount of atleast 10 wt. %, at least 15 wt. %, at least 20 wt. %, at least 25 wt. %,at least 30 wt. %, at least 40 wt. %, at least 50 wt. %, at least 60 wt.%, at least 70 wt. %, at least 80 wt. %, at least 90 wt. %, or even atleast 95 wt of the total mass of the fluid stream.

In other embodiments, the fluid stream contains little or no combustiblegas species. The fluid stream may not be chemically reactive with thefeed stream. For example, the feeds stream may comprise, consistessentially of, or consist of inert gases such as nitrogen. In one ormore embodiments, the fluid stream may comprise inert gas, such asnitrogen, in an amount of at least 5 wt. % of the total mass of thefluid stream. In additional embodiments, the fluid stream may compriseoxygen in an amount of at least 10 wt. %, at least 15 wt. %, at least 20wt. %, at least 25 wt. %, at least 30 wt. %, at least 40 wt. %, at least50 wt. %, at least 60 wt. %, at least 70 wt. %, at least 80 wt. %, atleast 90 wt. %, or even at least 95 wt of the total mass of the fluidstream. In additional embodiments, the fluid stream may comprise oxygenin an amount of less than or equal to 10 wt. % of the total mass of thefluid stream. For example, the fluid stream may comprise oxygen in anamount of less than or equal to 7.5 wt. %, less than or equal to 5 wt.%, less than or equal to 4 wt. %, less than or equal to 3 wt. %, lessthan or equal to 2 wt. %, or even less than or equal to 1 wt. % of thetotal mass of the fluid stream.

The fluid stream may be at an ambient temperature, or may be heated toan elevated temperature. According to various embodiments, the fluidstream may be heated and have a temperature of at least 100° F., atleast 150° F., at least 200° F., at least 250° F., at least 300° F., atleast 350° F., at least 400° F., at least 450° F., at least 500° F., atleast 550° F., at least 600° F., at least 650° F., at least 700° F., atleast 750° F., at least 800° F., at least 850° F., at least 900° F., atleast 950° F., at least 1000° F., at least 1050° F., at least 1100° F.,at least 1150° F., at least 1200° F., at least 1250° F., at least 1300°F., at least 1350° F., at least 1400° F., at least 1450° F., or even atleast 1500° F. For example, the fluid stream may have a temperature offrom 400° F. to 900° F., such as from 500° F. to 800° F., from 600° F.to 700° F., or from 500° F. to 650° F. In other embodiments, the fluidstream may have a temperature of from about 0° F. to 100° F., such asfrom 50° F. to 90° F., or from 60° F. to 80° F.

The fluid stream may have a superficial velocity of from 100 ft/s to2500 ft/s. For example, the superficial velocity of the fluid stream maybe at least 200 ft/s, at least 500 ft/s, at least 1000 ft/s, at least1500 ft/s, or at least 2000 ft/s, such as from 100 ft/s to 300 ft/s,from 300 ft/s to 500 ft/s, from 500 ft/s to 1000 ft/s, from 1000 ft/s to2000 ft/s, or from 2000 ft/s to 2500 ft/s.

As described herein, the feed stream is passed through the first conduit810 of the multi-conduit reactor 800 and the fluid stream is passedthrough the second conduit 830 of the multi-conduit reactor 800, wherethe feed stream and the fluid stream contact one another in the mixingzone 870. In one or more embodiments, the contacting of the fluid streamwith the feed stream may atomize some or all materials of the feedstream.

In one or more embodiments, the characteristics of the atomization ofthe materials in the feed stream may be a function of the momentum fluxratio. For example, the particle size may be correlated to the momentumflux ratio. As used herein, the momentum flux ratio is the ratio of themomentum flux of the fluid stream to the momentum flux of the feedstream. The momentum flux ratio can be represented by Equation 1, whereM represents the momentum flux ratio, ρ_(fluid) is the density of thefeed stream, U_(Fluid) is the superficial velocity of the feed stream,PFeed is the density of the feed stream, and U_(Feed) is the superficialvelocity of the feed stream.

$\begin{matrix}{M = \frac{\rho_{Fluid}U_{Fluid}^{2}}{\rho_{Feed}U_{Feed}^{2}}} & {{Equation}\mspace{14mu} 1}\end{matrix}$

Without being bound by any particular theory, the momentum flux ratiomay be correlated to the characteristics of the atomization by the Weiss& Worsham model (available in the publication by Malcom Weiss andCharles Worsham, entitled Atomization in High Velocity Airstreams, EssoResearch and Engineering Co., Linden N.J., 1959), allowing for a desiredatomization to be achieved by selection of the superficial velocity ofthe feed stream and the superficial velocity of the fluid stream.However, it should be understood that other models may be suitable forvarious reactor geometries and designs, where the Reynolds Number and/orWeber Number of one or more of the streams varies. According to one ormore embodiments, the momentum flux ratio may be from 0.3 to 48. Inadditional embodiments, the momentum flux ratio may be from 0.1 to 100,such as from 0.1 to 1, from 1 to 5, from 5 to 25, from 25 to 50, from 50to 75, or from 75 to 100.

According to one or more embodiments, the feed stream may be atomizedinto droplets having a Sauter Mean Diameter of less than or equal to 1mm. For example, the Sauter Mean Diameter of the atomized droplets maybe less than or equal to 750 microns, less than or equal to 500 microns,less than or equal to 250 microns, or even less than or equal to 100microns, such as from 1 micron to 25 microns, from 25 microns to 100microns, from 100 microns to 500 microns, from 500 microns to 1000microns, or from 10 micron to 15 microns.

The contacting of the feed stream with the fluid stream may also cause acombustion reaction, particularly in embodiments where the fluid streamcomprises oxygen. The combustion reaction may form metal oxides from theone or more metals or alloys of the feed stream. The oxidation of thesemetals or alloys may be exothermic, and may release heat sufficient tomaintain a flame temperature in the mixing zone 870 of the multi-conduitreactor 800 which allows for the perpetual continuation of thecombustion reaction. The flame temperature may be greater than themelting point of the metal or alloy in the feed stream (or even muchgreater than (e.g., at least 100° F. greater than) the melting point ofthe metal or alloy in the feed stream, but within the operatingtemperatures permitted by the materials of the multi-conduit reactor800. Additionally, in the flame temperature may be below a temperaturewhich would form oxides of nitrogen.

According to some embodiments, the flame temperature in the mixing zone870 may be a function of the ratio of gas from the fluid stream to metalor metal alloy from the feed stream. Since the flame temperature may becontrolled by adjusting the ratio of gas from the fluid stream to metalor metal alloy from the feed stream, the ratio of gas from the fluidstream to metal or metal alloy from the feed stream may be selected suchthat the flame temperature meets the operation parameters discussedherein, such as being greater than the melting point of the metal butless than a temperature not suitable for the materials of the reactorand a temperature which oxidizes nitrogen. For example, if lead iscontained in the feed stream, the ratio of gas from the fluid stream tolead in the feed stream may be from 0.3 to 4.5, such as from 0.4 to0.65, such that the flame temperature is from 1700° F. to 3000° F. FIG.14 depicts an example relationship between the flame temperature and theratio of gas to metal. According to one or more additional embodiments,the ratio of gas from the fluid stream to metal or metal alloy from thefeed stream may be from 0.25 to 10, such as from 0.25 to 1, from 1 to 2,from 2 to 4, from 4 to 6, from 6 to 8, or from 8-10. As describedherein, the ratio of gas from the fluid stream to metal or metal alloyfrom the feed stream is a weight basis measurement.

In addition to the ratio of oxygen to metal, in some embodiments, thetemperature of the feed stream and/or the temperature of the fluidstream may affect the flame temperature. In general, the flametemperature may rise with increasing feed stream temperatures and/orincreasing fluid stream temperatures. FIG. 15 depicts an examplerelationship between the flame temperature and the feed streamtemperature. Moreover, FIG. 16 depicts the momentum ratio when plottedagainst pressure, where each line represents a liquid molten metalvelocity. The lead velocity has a significant impact on momentum ratiobase on the data of FIG. 16. As such, in some embodiments, about 5 ft/smolten metal velocity may be desirable so that momentum ratio ismaximized while the flowrate of molten metal is still reasonable high.

In one or more embodiments, the ratio of the mass flowrate of the feedstream to the mass flowrate of the fluid stream may be from 0.05 to 0.5,such as from 0.2 to 0.3, from 0.3 to 0.4, or from 0.4 to 0.5.

In some embodiments, the multi-conduit reactor 800 may comprise asupplemental heating source in the mixing zone. The supplemental heatingsource may be utilized to ignite the combustion reaction. Once thecombustion reaction begins, the flame temperature may be held withoutsupplemental heating as long as adequate fuel (i.e., the metal or alloyfrom the feed stream) and oxygen is supplied. The supplemental heatingsource may comprise one or more of an ignition system, a burner, or anyother apparatus suitable for supplying heat or a flame.

According to additional embodiments, a quench stream may enter themixing zone 870 via the third conduit 850 and react with the componentsof the feed stream. Without being bound by theory, the quench stream maychange one or more characteristics of the metal or metal oxide in theproduct stream, and may aid in cooling the product stream to atemperature below the melting point of the metal or alloy in the productstream, forming solids. The quench stream may alter the crystalstructure of the components of the product stream. Without being boundby theory, it is believed that the rate of cooling of the product streammay affect the crystal structure of the metal, alloy, or metal oxide.The crystal structure may determine the color of the metal in the feedstream, so color of the product stream may be a controllable property insome embodiments.

In some embodiments, the quench stream may change the oxidation statethe metals in the product stream from what they would have been had thequench stream not been present. For example, a quench stream thatcomprises oxygen may raise the oxidation state of a metal in the productstream.

The quench stream may comprise one or more chemical species in a gasphase. According to some embodiments, the quench stream may comprise acombustible gas, such as oxygen. For example, the quench stream maycomprise, consist essentially of, or consist of air. In one or moreembodiments, the quench stream may comprise oxygen in an amount of atleast 5 wt. % of the total mass of the quench stream. In additionalembodiments, the quench stream may comprise oxygen in an amount of atleast 10 wt. %, at least 15 wt. %, at least 20 wt. %, at least 25 wt. %,at least 30 wt. %, at least 40 wt. %, at least 50 wt. %, at least 60 wt.%, at least 70 wt. %, at least 80 wt. %, at least 90 wt. %, or even atleast 95 wt. % of the total mass of the quench stream.

In other embodiments, the quench stream contains little or nocombustible gas species. The quench stream may not be chemicallyreactive with the feed stream. For example, the feeds stream maycomprise, consist essentially of, or consist of inert gases such asnitrogen. In one or more embodiments, the quench stream may compriseinert gas, such as nitrogen, in an amount of at least 5 wt. % of thetotal mass of the quench stream. In additional embodiments, the quenchstream may comprise oxygen in an amount of at least 10 wt. %, at least15 wt. %, at least 20 wt. %, at least 25 wt. %, at least 30 wt. %, atleast 40 wt. %, at least 50 wt. %, at least 60 wt. %, at least 70 wt. %,at least 80 wt. %, at least 90 wt. %, or even at least 95 wt of thetotal mass of the quench stream. In additional embodiments, the quenchstream may comprise oxygen in an amount of less than or equal to 10 wt.% of the total mass of the quench stream. For example, the quench streammay comprise oxygen in an amount of less than or equal to 7.5 wt. %,less than or equal to 5 wt. %, less than or equal to 4 wt. %, less thanor equal to 3 wt. %, less than or equal to 2 wt. %, or even less than orequal to 1 wt. % of the total mass of the quench stream.

The quench stream may be at an ambient temperature, or may be heated toan elevated temperature. In some embodiments, the quench stream may havea temperature of from about 0° F. to 100° F., such as from 50° F. to 90°F., or from 60° F. to 80° F. In some embodiments, the quench stream maybe ambient air or cooled air.

In other embodiments, the quench stream may be heated and have atemperature of at least 100° F., at least 150° F., at least 200° F., atleast 250° F., at least 300° F., at least 350° F., at least 400° F., atleast 450° F., at least 500° F., at least 550° F., at least 600° F., atleast 650° F., at least 700° F., at least 750° F., at least 800° F., atleast 850° F., at least 900° F., at least 950° F., at least 1000° F., atleast 1050° F., at least 1100° F., at least 1150° F., at least 1200° F.,at least 1250° F., at least 1300° F., at least 1350° F., at least 1400°F., at least 1450° F., or even at least 1500° F. In additionalembodiments, the quench stream may have a temperature of from −20° F. to150° F.

In one or more embodiments, the quench stream may have a pressure of atleast 15 psia. For example, the quench stream may have a pressure of atleast 20 psia, at least 30 psia, at least 40 psia, or even at least 50psia, such as from 15 psia to 100 psia, from 30 psia to 100 psia, orfrom 50 psia to 100 psia.

The quench stream may have a superficial velocity of from 100 ft/s to2500 ft/s. For example, the superficial velocity of the quench streammay be at least 100 ft/s, at least 500 ft/s, at least 1000 ft/s, atleast 1500 ft/s, or at least 2000 ft/s, such as from 100 ft/s to 500ft/s, from 500 ft/s to 1000 ft/s, from 1000 ft/s to 1500 ft/s, from 1500ft/s to 2000 ft/s, or from 2000 ft/s to 2500 ft/s.

The quench stream may have a mass flowrate of from 0.05 lbs/s to 50lbs/s. For example, the mass flowrate of the quench stream may be atleast 0.05 lbs/s, at least 0.5 lbs/s, at least 1 lbs/s, at least 5lbs/s, or at least 10 lbs/s, such as from 0.05 lbs/s to 0.5 lbs/s, from0.5 lbs/s to 1 lbs/s, from 1 lbs/s to 10 lbs/s, from 10 lbs/s to 30lbs/s, or from 30 lbs/s to 50 lbs/s. For example, the quench stream mayhave a mass flowrate of from 0.2 lbs/s to 0.5 lbs/s

The resulting components following the contacting of the feed stream andthe fluid stream form a product stream, which exits the multi-conduitreactor. The product stream may comprise one or more powdered metals oralloys, or oxides thereof. According to one embodiment, if one or moreof the fluid stream or the quench stream comprises oxygen, a metal oxidemay be present in the product stream. Without being bound by theory, asdisclosed above, it is believed that the size of the particles of thepowder of the product stream may be a function of the momentum fluxratio, as explained previously in this disclosure. The metal, alloy, oroxide particles present in the product stream may have the same orsimilar size as the liquefied, atomized droplets of the feed stream whenit is contacted by the fluid stream.

Having described the subject matter of the present disclosure in detailand by reference to specific embodiments, it is noted that the variousdetails described in this disclosure should not be taken to imply thatthese details relate to elements that are essential components of thevarious embodiments described in this disclosure, even in cases where aparticular element is illustrated in each of the drawings that accompanythe present description. Rather, the claims appended hereto should betaken as the sole representation of the breadth of the presentdisclosure and the corresponding scope of the various embodimentsdescribed in this disclosure. Further, it will be apparent thatmodifications and variations are possible without departing from thescope of the appended claims.

What is claimed is:
 1. A method for forming metal-containing particles,the method comprising: forming a molten material from a solid supplymaterial; introducing the molten material into a reaction zone of aBarton reactor, the Barton reactor comprising a reaction vesselcomprising a top cover and sidewalls defining the reaction zone, anagitator, a processing gas inlet, and a product outlet, wherein themolten material is introduced to the reaction zone in a laminar flow oras atomized molten particles; and contacting the molten material with aprocessing gas in the reaction zone to form solid metal-containingparticles comprising solid metallic particles and solid metal oxideparticles, wherein less than 99% of the particles comprise metal oxide.2. The method of claim 1, wherein the formed metal-containing particlesinclude lead oxide particles and lead metal particles, and wherein theweight ratio of formed lead oxide particles to lead metal particles isless than 99:1
 3. The method of claim 2, wherein the weight ratio offormed solid lead oxide particles to solid lead metal particles is from50:50 to 90:10.
 4. The method of claim 2, wherein the reaction zone hasa temperature of from 621° F. to 880° F.
 5. The method of claim 2,wherein the majority by weight of solid lead oxide particles comprisealpha lead oxide having a tetragonal crystal structure, and wherein theparticles are suitable for lead acid battery manufacturing.
 6. Themethod of claim 1, wherein the weight ratio of formed solid lead oxideparticles to solid lead metal particles is from 50:50 to 90:10, andwherein the majority by weight of solid lead oxide particles comprisealpha lead oxide having a tetragonal crystal structure.
 7. The method ofclaim 1, wherein at least 99% of the particles are non-oxidized metals,metalloids, or alloys.
 8. The method of claim 1, wherein the moltenmetal lead material is introduced into the reaction zone in a hollowconical laminar spray.
 9. The method of claim 1, wherein the moltenmetal lead material is introduced into the reaction zone in an atomizedform.
 10. The method of claim 1, wherein the molten metal lead materialis introduced into the reaction zone through a nozzle.
 11. The method ofclaim 1, wherein the processing gas is an oxidizing agent such asoxygen, air, or combinations thereof.
 12. The method of claim 1, whereinthe formed metal-containing particles include lead oxide particles andlead metal particles, and wherein the weight ratio of formed lead oxideparticles to lead metal particles is from 50:50 to 90:10, and wherein atleast 90 wt. % of solid lead oxide particles comprise alpha lead oxidehaving a tetragonal crystal structure.
 13. A method for retrofitting aBarton reactor, the method comprising: replacing a conventional moltenmaterial inlet of a Barton reactor with an injector operable to receivemolten material and inject the molten material into a reaction zone ofthe Barton reactor; wherein the injector is operable to pass moltenmetal-containing material into the reaction zone with a laminar flow orin an atomized form.
 14. The method of claim 13, wherein theconventional molten material inlet comprises a pipe.
 15. The method ofclaim 13, wherein the conventional molten material inlet comprises atrough, dam, lip, or like device.
 16. The method of claim 13, whereinthe injector comprises a nozzle.
 17. the method of claim 13, wherein theinjector is operable to pass the molten metal-containing material intothe reaction zone with a laminar flow.
 18. The method of claim 13,wherein the injector is operable to pass the molten metal-containingmaterial into the reaction zone in an atomized form.
 19. The method ofclaim 13, further comprising operating the retrofitted Barton reactor toform lead metal particles, lead oxide particles, or a mixture thereof.20. The method of claim 19, wherein the operation of the retrofittedBarton reactor forms a mixture of lead metal particles and lead oxideparticles suitable for use in a lead acid battery, and wherein theretrofitted Barton reactor is operated at a temperature of from 621° F.to 880° F.